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The synergistic effect of bimetallic heterogeneous catalysis in the reaction of nitrate reduction to nitrogen has been widely discussed, but it is still not clear how this effect works at the atomic scale, hindering the rational design of high‐performance catalysts. Here, for the first time, 2D phosphorene was used as a giant P ligand to confine high‐density PdCu dual‐atom to form a unique PdCuP4...
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